The micro-mesoporous TS-1 catalyst was synthesized by directly introducing NaOH during the synthesis of zeolite. As the first choice for many oxidation reactions, TS-1/HO catalytic system is an environmentally friendly reaction system. However, the number and mechanism of Ti active sites participating in the reaction in TS-1 zeolite are seldom studied so far. Using TS-1 zeolite with and without NaOH as catalyst, -diethylbenzene (PDEB) was oxidized in batch reactor to prepare -ethylacetophenone and 1-(4-ethylphenyl)-1-ethanol. Reaction conditions including solvent, additives, temperature, time, dosage and oxidant were explored. The optimum reaction conditions, the conversion of PDEB was 27.7 % and the total selectivity was 74.5 % over TS-1-NaOH zeolite catalyst, where the selectivity of -ethylacetophenone and 4-ethyl-α-methylbenzyl alcohol was 33.4 % and 41.1 %, respectively. Introducing mesoporous structure reduces the mass transfer resistance of the reaction and improves the selectivity of the target product. Based on the free radical reaction mechanism and the oxidative decomposition process of HO, it is inferred that the oxidation mechanism of PDEB in HO system is a free radical reaction with the participation of •O.

中文翻译：

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微介孔TS-1沸石的合成及其绿色催化氧化对二乙苯

在沸石合成过程中直接引入NaOH，合成了微介孔TS-1催化剂。 TS-1/H2O催化体系作为许多氧化反应的首选，是一种环境友好的反应体系。然而，目前对TS-1沸石中参与反应的Ti活性位点的数量和机理的研究还很少。以TS-1沸石为催化剂，在间歇式反应器中氧化邻二乙苯(PDEB)，制备邻乙基苯乙酮和1-(4-乙基苯基)-1-乙醇。探讨了反应条件，包括溶剂、添加剂、温度、时间、用量和氧化剂。最佳反应条件为,在TS-1-NaOH沸石催化剂上PDEB转化率为27.7%,总选择性为74.5%,其中β-乙基苯乙酮和4-乙基-α-甲基苯甲醇的选择性分别为33.4%和41.1%,分别。介孔结构的引入降低了反应的传质阻力，提高了目标产物的选择性。根据自由基反应机理和H2O的氧化分解过程，推测PDEB在H2O体系中的氧化机理是有·O参与的自由基反应。